Steering post-C-C coupling selectivity enables high efficiency electroreduction of carbon dioxide to multi-carbon alcohols
Steering post-C-C coupling selectivity enables high efficiency electroreduction of carbon dioxide to multi-carbon alcohols
复制标题
控制 C-C 偶联后的选择性可实现二氧化碳高效电还原为多碳醇
DOI：
10.1038/s41929-018-0084-7
复制
发表时间：
2018
期刊：
影响因子：
37.8
通讯作者：
Sinton Dav
中科院分区：
文献类型：
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作者：
Zhuang Tao-Tao;Liang Zhi-Qin;Seifitokaldani Ali;Li Yi;De Luna Phil;Burdyny Thomas;Che Fanglin;Meng Fei;Min Yimeng;Quintero-Bermudez Rafael;Cao Thang Dinh;Pang Yuanjie;Zhong Miao;Zhang Bo;Li Jun;Chen Pei-Ning;Liang Hongyan;Ge Wen-Na;Ye Bang-Jiao;Sinton Dav
考虑到这些液体燃料的能量密度、易于运输和已建立的用途，需要有利于高价值醇的工程铜基催化剂。在催化剂的设计中，针对C-C偶联步骤已经取得了很大的进展;而针对后C-C偶联反应中间体的努力相对较少。在这里，我们报告了一类核-壳空位工程催化剂，利用纳米颗粒核中的硫原子和壳中的铜空位，实现高效的电化学CO2还原为丙醇和乙醇。这些催化剂将选择性从竞争性乙烯反应转移到液体醇。与裸铜纳米颗粒相比，我们将醇与乙烯的比例提高了六倍以上，突出了电解醇而不是烯烃的替代方法。我们实现了126 ± 5 mA cm− 2的C2+醇生产速率，法拉第效率的选择性为32 ± 1%。
Engineering copper-based catalysts that favour high-value alcohols is desired in view of the energy density, ready transport and established use of these liquid fuels. In the design of catalysts, much progress has been made to target the C–C coupling step; whereas comparatively little effort has been expended to target post-C–C coupling reaction intermediates. Here we report a class of core–shell vacancy engineering catalysts that utilize sulfur atoms in the nanoparticle core and copper vacancies in the shell to achieve efficient electrochemical CO2reduction to propanol and ethanol. These catalysts shift selectivity away from the competing ethylene reaction and towards liquid alcohols. We increase the alcohol-to-ethylene ratio more than sixfold compared with bare-copper nanoparticles, highlighting an alternative approach to electroproduce alcohols instead of alkenes. We achieve a C2+alcohol production rate of 126 ± 5 mA cm−2with a selectivity of 32 ± 1% Faradaic efficiency.